enhance the Raman scattering. [2,3] This process is called surface enhanced Raman scattering (SERS). The enhancement factor (EF) of SERS substrates is known to result from both electromagnetic and chemical enhancement. [4] It is widely acknowledged that the electromagnetic enhancement of plasmonic structures is the main EF contribution. The EF can be estimated by EF | | | | laser 2 Raman, where E laser and E Raman represent the field enhancement at the excitation (laser) wavelength and reemission (Raman) wavelength. [4] The near-field of plasmonic nanostructures can be particularly strong, when the field is concentrated in very small volumes. These socalled hotspots can occur, e.g., at the sharp tips of nanocones [2b] or in the gaps between different structures in a plasmonic multimer. Thus, in order to boost the enhancement of local electromagnetic (EM) fields, nanostructures with gaps on the scale of few nanometers, such as homodimers, [5] heterodimers, [6] trimers, [7] and vertical metal-insulator-metal (MIM) structures [8] were investigated extensively.In the case of lateral dimers or oligomers, the hotspots in the gaps between the single structures are readily accessible for detecting molecules. However, narrow gaps smaller than 10 nm are of poor reproducibility limited by the resolution of e-beam lithography (EBL). [5] On the contrary, vertical MIM structures with gaps down to the sub-nanometer scale can be obtained with thin film techniques such as atomic layer deposition (ALD) with high tunability and reproducibility. [9] Furthermore, a reproducible realization of gaps larger than 5 nm can be readily obtained with sufficient accuracy of the film thickness by established techniques such as evaporation or sputtering. [10] Due to their advantages in terms of large field enhancement and a straightforward fabrication method, vertical MIM structures, which consist of ordered nanodisc arrays on a gold film, separated by a thin dielectric layer, have attracted great attention in scientific research. [8a,11] Many groups have been concentrating on the theory of cavity plasmon modes and concluded that these modes result from the interplay of plasmonic modes and Fabry-Pérot cavities defined by the MIM structure. [11a,b,e,12,13] The cavity plasmon modes in vertical MIM structures have been exploited in applications such as structural colors, [11a,b,d] photovoltaics, [13] narrow-band perfect absorbers, [14] enhancing the spontaneous emission rate of dyes, [15] and enhanced infrared absorption. [16] It has been widely shown that the cavity In metal-insulator-metal structures such as Au nanodiscs on an Au film separated by a thin oxide spacer layer, the metal/insulator interfaces can form a Fabry-Perot cavity in which gap surface plasmons are confined. As a result, these cavity plasmon modes show the advantageous properties of strong field enhancement and very narrow resonance line shapes due to the confinement in a cavity. In this work, the hotspots of the electromagnetic near-field of cavity plasmon modes ar...